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Title: The Chemistry of CO 2 Capture in an Amine-Functionalized Metal–Organic Framework under Dry and Humid Conditions

The use of two primary alkylamine functionalities covalently tethered to the linkers of IRMOF-74-III results in a material that can uptake CO 2 at low pressures through a chemisorption mechanism. In contrast to other primary amine-functionalized solid adsorbents that uptake CO2primarily as ammonium carbamates, we observe using solid state NMR that the major chemisorption product for this material is carbamic acid. The equilibrium of reaction products also shifts to ammonium carbamate when water vapor is present; a new finding that has impact on control of the chemistry of CO 2 capture in MOF materials and one that highlights the importance of geometric constraints and the mediating role of water within the pores of MOFs.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [3] ; ORCiD logo [1] ;  [1] ;  [4] ;  [1] ;  [5] ; ORCiD logo [6]
  1. Department of Chemistry, University of California−Berkeley, Materials Sciences Division, Lawrence Berkeley National Laboratory, Kavli Energy NanoSciences Institute at Berkeley, and Berkeley Global Science Institute, Berkeley, California 94720, United States
  2. Department of Chemistry, University of California−Berkeley, Materials Sciences Division, Lawrence Berkeley National Laboratory, Kavli Energy NanoSciences Institute at Berkeley, and Berkeley Global Science Institute, Berkeley, California 94720, United States; Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States
  3. Department of Chemistry, University of California−Berkeley, Materials Sciences Division, Lawrence Berkeley National Laboratory, Kavli Energy NanoSciences Institute at Berkeley, and Berkeley Global Science Institute, Berkeley, California 94720, United States; Instituto de Investigaciones en Fisicoquímica de Córdoba, INFIQC−CONICET, Facultad de Ciencias Químicas, Departamento de Química Orgánica, Universidad Nacional de Córdoba, Ciudad Universitaria, X5000HUA Córdoba, Argentina
  4. King Abdulaziz City for Science and Technology (KACST), Riyadh 11442, Saudi Arabia
  5. Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  6. Department of Chemistry, University of California−Berkeley, Materials Sciences Division, Lawrence Berkeley National Laboratory, Kavli Energy NanoSciences Institute at Berkeley, and Berkeley Global Science Institute, Berkeley, California 94720, United States; King Abdulaziz City for Science and Technology (KACST), Riyadh 11442, Saudi Arabia
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 35; Related Information: © 2017 American Chemical Society.; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
OSTI Identifier:
1464153